CN101351917B - Fuel cell and fuel cell stack - Google Patents

Fuel cell and fuel cell stack Download PDF

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Publication number
CN101351917B
CN101351917B CN2006800497836A CN200680049783A CN101351917B CN 101351917 B CN101351917 B CN 101351917B CN 2006800497836 A CN2006800497836 A CN 2006800497836A CN 200680049783 A CN200680049783 A CN 200680049783A CN 101351917 B CN101351917 B CN 101351917B
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China
Prior art keywords
fuel gas
fuel
oxygen
dividing plate
channel
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CN101351917A (en
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锺尾幸久
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Honda Motor Co Ltd
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Honda Motor Co Ltd
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0247—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the form
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/2404—Processes or apparatus for grouping fuel cells
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/241—Grouping of fuel cells, e.g. stacking of fuel cells with solid or matrix-supported electrolytes
    • H01M8/2425—High-temperature cells with solid electrolytes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/241—Grouping of fuel cells, e.g. stacking of fuel cells with solid or matrix-supported electrolytes
    • H01M8/2425—High-temperature cells with solid electrolytes
    • H01M8/243—Grouping of unit cells of tubular or cylindrical configuration
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/241—Grouping of fuel cells, e.g. stacking of fuel cells with solid or matrix-supported electrolytes
    • H01M8/2425—High-temperature cells with solid electrolytes
    • H01M8/2432—Grouping of unit cells of planar configuration
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/2457—Grouping of fuel cells, e.g. stacking of fuel cells with both reactants being gaseous or vaporised
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/2465—Details of groupings of fuel cells
    • H01M8/2483—Details of groupings of fuel cells characterised by internal manifolds
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/2465—Details of groupings of fuel cells
    • H01M8/2484—Details of groupings of fuel cells characterised by external manifolds
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

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  • Life Sciences & Earth Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Fuel Cell (AREA)

Abstract

A fuel cell (11) includes a separator (28) having a circular disk (36). On one surface (36a) of the circular disk (36), a fuel gas channel (46) for supplying a fuel gas to an anode (24) is provided, and on the other surface (36b) of the circular disk (36), an oxygen-containing gas channel (70) for supplying air to a cathode (22) is provided. The fuel gas channel (46) has an end point disposed at the outer circumferential end of the anode (24). A fuel gas discharge channel (68) is connected to the end point of the fuel gas channel (46), such that the consumed fuel gas is emitted from a position spaced outwardly from an outer circumferential portion of the electrolyte electrode assembly (26).

Description

Fuel cell and fuel battery
Technical field
The present invention relates to a kind of by piling up the fuel cell that electrolyte membrane-electrode assembly and dividing plate form.Electrolyte membrane-electrode assembly comprise anode, negative electrode and be plugged in anode and negative electrode between electrolyte.In addition, the present invention relates to a kind of by piling up the fuel battery that a plurality of fuel cells form.
Background technology
Usually, the Solid Oxide Fuel Cell (SOFC) with no seal (not having sealing) structure adopts the electrolyte that is made of the ionic conduction soild oxide such as stabilizing zirconia.Electrolyte is plugged between anode and the negative electrode to form electrolyte membrane-electrode assembly.Electrolyte membrane-electrode assembly is plugged between the dividing plate (bipolar plates).In use, electrolyte membrane-electrode assembly and the dividing plate with predetermined quantity is stacked to form fuel battery.
The working temperature of fuel cell is higher, is approximately 800 ℃.Therefore, the zone around the fuel gas that will consume (hereinafter be also referred to as waste gas, contain the reacting gas that does not consume in the waste gas) is discharged to fuel battery and mixes with oxygen-containing gas and cause that when burning, the temperature part of fuel battery is higher.In these cases, fuel battery can not stably be worked.In addition, the water that produces during burning contacts with heated dividing plate is local, causes the dividing plate corrosion.As a result, the durability of dividing plate reduces.And, in electrolyte membrane-electrode assembly, specifically be that the anode of localized heating is oxidized.Thereby in electrolyte membrane-electrode assembly, break, and performance inconsistency deterioration desirably.
In this respect, known a kind of as the disclosed Solid Oxide Fuel Cell of Japanese laid-open patent communique No.2005-85520.As shown in figure 24, this fuel cell forms by piling up generating battery 1, fuel electrode current-collector 2, air electrode current-collector 3 and dividing plate 4a, 4b.Generating battery 1 comprise fuel electrode layer 1b, air electrode layer 1c and be plugged in fuel electrode layer 1b and air electrode layer 1c between solid electrolyte layer 1a.Fuel electrode current-collector 2 is arranged on the outside of fuel electrode layer 1b, and air electrode current-collector 3 is arranged on the outside of air electrode layer 1c.
Dividing plate 4a comprises fuel gas channel 5, and fuel gas channel 5 is used for roughly from the core fuel supplying gas towards the surface of the dividing plate 4a of fuel electrode current-collector 2.Dividing plate 4b has oxygen-containing gas passage 6, and oxygen-containing gas passage 6 is used for roughly from the core supply oxygen-containing gas towards the dividing plate 4b of air electrode current-collector 3.
Though not shown, endless metal lid has covered the peripheral part of circular porous metal bodies, wherein is provided with a large amount of steam vent 7 on the whole sidepiece of lid.
In this structure, gas is only discharged by steam vent 7 from the peripheral part of fuel electrode current-collector 2.Thereby fuel gas is diffused in the porous metal bodies and does not overflow from the whole peripheral part of fuel electrode current-collector 2.According to the disclosure, suppressed during generating electricity, not have to use and the amount of the fuel gas of discharging from peripheral part, thereby can prevent that air is towards the fuel electrode diffuse in reverse direction.
Yet in above conventional art, dividing plate 4a is stacked on the fuel electrode current-collector 2, and the exhaust of discharging from steam vent 7 is burnt near dividing plate 4a whereby, thereby produces water.Thereby, dividing plate 4a and generating battery 1 local heating, and be tending towards damaging easily owing to steam oxidation.Also may corrode, this can make the fuel cell performance deterioration wastefully.
Summary of the invention
In order to handle and to address the above problem, the object of the present invention is to provide fuel cell simple in structure and fuel battery, can prevent reliably that wherein electrolyte membrane-electrode assembly from contacting with the water vapour that during reaction produces with dividing plate, thereby prevent damage effectively electrolyte membrane-electrode assembly and dividing plate.
The present invention relates to a kind of by piling up the fuel cell that electrolyte membrane-electrode assembly and dividing plate form.This electrolyte membrane-electrode assembly comprises anode, negative electrode and is plugged in electrolyte between described anode and the negative electrode.On a surface of described dividing plate, be formed for, and on another surface of described dividing plate, be formed for along the oxygen-containing gas passage of the surface supply oxygen-containing gas of described negative electrode along the fuel gas channel of the surperficial fuel supplying gas of described anode.
Described fuel gas channel has the terminal point that is positioned at the position corresponding with the peripheral part of described electrolyte membrane-electrode assembly, this terminal point of wherein said fuel gas channel is connected to fuel gas discharge channel, and this fuel gas discharge channel makes the fuel gas that consumes in described electrolyte membrane-electrode assembly from overflowing with the outside position spaced of the peripheral part of this electrolyte membrane-electrode assembly.Described fuel gas discharge channel comprises the through hole that connects described dividing plate extension, and another lip-deep letdown tank parts that are arranged on described dividing plate, and described letdown tank parts are connected to described through hole and stretch out from described electrolyte membrane-electrode assembly.
Preferably, described fuel gas channel comprises a lip-deep channel unit that is arranged on described dividing plate, and wherein this channel unit is connected to described fuel gas discharge channel from fuel gas inlet.
In addition preferably, described fuel gas discharge channel is formed by letdown tank and cover, described letdown tank is arranged on the surface of described dividing plate and is connected to described fuel gas channel, and described cover is arranged on the surface of described dividing plate to cover described letdown tank.
In addition preferably, the annular projection that closely contacts with the peripheral part of described anode is set on a surface of described dividing plate.By this structure, can prevent that exhaust from entering (comprising the fuel gas of consumption and the oxygen-containing gas of consumption) peripheral part of described anode, can prevent described anode whereby because oxidation and deterioration.
In addition preferably, described channel unit forms by groove, a plurality of projection or with deformable elastic passage component that described anode closely contacts.
In addition preferably, described oxygen-containing gas passage is gone up by another surface that is arranged on described dividing plate and is formed with deformable elastic passage component that described negative electrode closely contacts.By this structure, described negative electrode suitably closely contacts with described dividing plate, thereby has improved from the performance of fuel cell current collection.
In addition preferably, arrange the power generation region of the zone of described resilient channels parts less than described anode.In this structure,, in the neighboring relative described negative electrode, there is not power generation region with neighboring described anode even air exhaust loop flow to the anode of described electrolyte membrane-electrode assembly yet.Thereby can prevent the current collection loss, improve whereby from the performance of fuel cell current collection.
In addition preferably, described resilient channels parts are conduction mesh members or felt parts.In this case, can provide simplification and economic structure.
In addition preferably, described oxygen-containing gas passage is formed by another lip-deep a plurality of projections that are arranged on described dividing plate.Transmit effectively by described projection along the load that stacking direction applies, improved whereby from the performance of fuel cell current collection.
In addition preferably, described projection is made of a plurality of solid portions that form by etching on a surface of described dividing plate.Thereby the shape of described projection and position can easily change arbitrarily, have improved whereby from the performance of fuel cell current collection.
Preferably, described fuel cell also comprises the exhaust passage, and fuel gas and oxygen-containing gas that this exhaust passage is used for consuming at described electrolyte membrane-electrode assembly between the stage of reaction discharge as the stacking direction of exhaust along described electrolyte membrane-electrode assembly and described dividing plate.In addition, the oxygen-containing gas feeding unit is set, is used for oxygen-containing gas is fed to the oxygen-containing gas passage along stacking direction as the path of oxygen-containing gas before consuming.The fuel gas feeding unit is provided with airtightly with respect to described oxygen-containing gas feeding unit, wherein the fuel gas service duct connects described fuel gas channel and described fuel gas feeding unit, thereby and crossing with the oxygen-containing gas feeding unit that extends along stacking direction along the surface arrangement of described dividing plate.In this structure, the heat that fuel gas was deflated before consuming heats in advance.Thereby improved the heat efficiency.
In addition preferably, described exhaust passage is arranged on around the described dividing plate.In this structure, around fuel cell, provide adiabatic, improved the heat efficiency whereby.
Preferably, described fuel gas feeding unit is arranged on the core of described dividing plate airtightly, and described oxygen-containing gas feeding unit is arranged on the interior zone of described dividing plate.In this structure, oxygen-containing gas outwards flows from the interior zone of described dividing plate.Therefore, exhaust suitably is discharged into the outside of described dividing plate.In addition preferably, described fuel gas inlet is arranged on the center of described electrolyte membrane-electrode assembly.
Preferably, described fuel cell also comprises the exhaust passage, and fuel gas and oxygen-containing gas that this exhaust passage is used for consuming at described electrolyte membrane-electrode assembly between the stage of reaction discharge as the stacking direction of exhaust along described electrolyte membrane-electrode assembly and described dividing plate.In addition, the oxygen-containing gas feeding unit is set, this oxygen-containing gas feeding unit is used for oxygen-containing gas is fed to the oxygen-containing gas passage along stacking direction as the path of oxygen-containing gas before consuming.Described fuel gas feeding unit and described oxygen-containing gas feeding unit are arranged in the described exhaust passage airtightly, wherein said fuel gas service duct connects described fuel gas channel and described fuel gas feeding unit, thereby it is and crossing with the exhaust passage of extending along stacking direction along the surface arrangement of described dividing plate, and wherein said oxygen-containing gas service duct connects described oxygen-containing gas passage and described oxygen-containing gas feeding unit, thereby and crossing with described exhaust passage along the surface arrangement of described dividing plate.
In addition preferably, described fuel gas channel forms the fuel gas pressure chamber, make and when fuel gas is fed to described fuel gas channel, push described anode, and described oxygen-containing gas passage forms oxygen-containing gas pressure chamber, makes to push described negative electrode when oxygen-containing gas is fed to described oxygen-containing gas passage.
In addition preferably, a plurality of electrolyte membrane-electrode assemblies are arranged around the centres of described dividing plate.Thereby described fuel cell is of compact construction, and can avoid the influence of the thermal deformation on it whereby.
In addition, the present invention relates to a kind ofly by piling up the fuel battery that a plurality of fuel cells form, each fuel cell is by piling up electrolyte membrane-electrode assembly and dividing plate forms.This electrolyte membrane-electrode assembly comprises anode, negative electrode and is plugged in electrolyte between described anode and the negative electrode.On a surface of described dividing plate, be formed for, and on another surface of described dividing plate, be formed for along the oxygen-containing gas passage of the surface supply oxygen-containing gas of described negative electrode along the fuel gas channel of the surperficial fuel supplying gas of described anode.On a surface of described dividing plate or another surface, the fuel gas service duct is set, wherein this fuel gas service duct is connected to fuel gas provided the fuel gas feeding unit of path before consuming, and is provided for fuel gas is fed to fuel gas inlet in the described fuel gas channel.
Described fuel gas channel has the terminal point that is arranged in the position corresponding with the peripheral part of described electrolyte membrane-electrode assembly, the terminal point of wherein said fuel gas channel is connected to fuel gas discharge channel, and this fuel gas discharge channel makes the fuel gas that consumes in described electrolyte membrane-electrode assembly from overflowing with the outside position spaced of the peripheral part of this electrolyte membrane-electrode assembly.And described fuel gas discharge channel comprises the through hole that connects described dividing plate extension, and another lip-deep letdown tank parts that are arranged on described dividing plate, and described letdown tank parts are connected to described through hole and stretch out from described electrolyte membrane-electrode assembly.
Be fed to described anode with after carrying out electric power generation reaction at fuel gas, when fuel gas during as exhaust emissions, comprises the gas that does not consume from described anode in the exhaust.The exhaust that comprises this not spent gas is called waste gas.
According to the present invention, after fuel gas consumed in described electrolyte membrane-electrode assembly, waste gas was from overflowing with the outside position spaced of the peripheral part of described electrolyte membrane-electrode assembly.Thereby, can prevent that described electrolyte membrane-electrode assembly and described dividing plate are owing to the reaction of waste gas and oxygen-containing gas is locally heated high temperature.In addition, described electrolyte membrane-electrode assembly and described dividing plate not can with during reaction contact with water generates.
Thereby, can prevent reliably because the corrosion that causes of steam oxidation, thereby can improve the durability of described dividing plate.In addition, can prevent the oxidation of the oxidation of described electrolyte membrane-electrode assembly, particularly described anode.So, can prevent the impaired or deterioration of performance of described electrolyte membrane-electrode assembly.
Description of drawings
Fig. 1 is that expression comprises the partial sectional view according to the fuel cell system of the fuel cell of first embodiment of the invention;
Fig. 2 is the stereogram that schematically shows the fuel battery of fuel cell system;
Fig. 3 is the exploded perspective view of the fuel cell of expression fuel battery;
Fig. 4 is the exploded stereogram of the gas flow in the expression fuel cell;
Fig. 5 is the partial enlarged drawing on a surface of expression dividing plate;
Fig. 6 is another surperficial view of expression dividing plate;
Fig. 7 is the cutaway view that schematically shows the operation of fuel cell;
Fig. 8 is the view of another structure of expression fuel gas discharge channel;
Fig. 9 is the exploded perspective view of expression according to the fuel cell of second embodiment of the invention;
Figure 10 is the front view of the dividing plate of expression fuel cell;
Figure 11 is the cutaway view that schematically shows the operation of fuel cell;
Figure 12 is the exploded perspective view of expression according to the fuel cell of third embodiment of the invention;
Figure 13 is the partial enlarged drawing on a surface of expression dividing plate;
Figure 14 is the cutaway view that schematically shows the operation of fuel cell;
Figure 15 is the exploded perspective view of expression according to the fuel cell of four embodiment of the invention;
Figure 16 is the cutaway view that schematically shows the operation of fuel cell;
Figure 17 is the exploded perspective view of expression according to the fuel cell of fifth embodiment of the invention;
Figure 18 is the cutaway view that schematically shows the operation of fuel cell;
Figure 19 is the stereogram that schematically shows the fuel battery that forms by stacking fuel cells according to sixth embodiment of the invention;
Figure 20 is the exploded perspective view of expression fuel cell;
Figure 21 is the front view of expression fuel cell;
Figure 22 cuts open the cutaway view of getting along the line XXII-XXII among Figure 21;
Figure 23 is the exploded perspective view of expression according to the fuel cell of seventh embodiment of the invention; And
Figure 24 is the view of expression conventional fuel cell.
Embodiment
Fig. 1 is that expression comprises the partial sectional view according to the fuel cell system 10 of the fuel cell 11 of first embodiment of the invention.Fig. 2 schematically shows by pile up the stereogram of the fuel battery 12 that a plurality of fuel cells 11 form along direction shown in the arrow A.
Fuel cell system 10 is used in the various application, comprises fixation application and moves application.For example, fuel cell system 10 can be installed on the vehicle.As shown in Figure 1, fuel cell system 10 comprises fuel battery 12, heat exchanger 14, reformer 16 and housing 18.Before oxygen-containing gas is supplied to fuel battery 12, heat exchanger 14 these oxygen-containing gass of heating.Reformer 16 fuel reformings are to produce fuel gas.Fuel battery 12, heat exchanger 14 and reformer 16 are arranged in the housing 18.
In housing 18, on a side of fuel battery 12, arrange the element of fluid 19 that comprises heat exchanger 14 and reformer 16 at least, and on the opposite side of fuel battery 12, arrange the load applying mechanism 21 that is used for applying to fuel cell 11 fastening load along the stacking direction shown in the arrow A.Element of fluid 19 and load applying mechanism 21 are provided with symmetrically about the central axis of fuel battery 12.
Fuel cell 11 is Solid Oxide Fuel Cell (SOFC).As shown in Figure 3 and Figure 4, fuel cell 11 comprises electrolyte membrane-electrode assembly 26.Each electrolyte membrane-electrode assembly 26 include negative electrode 22, anode 24 and be plugged in negative electrode 22 and anode 24 between electrolyte (electrolyte panel) 20.For example, electrolyte 20 is made by the ionic conduction soild oxide such as stabilizing zirconia.Electrolyte membrane-electrode assembly 26 has disc-shape.The barrier layer (not shown) is set on the neighboring of electrolyte membrane-electrode assembly 26 at least, is used to prevent the turnover of oxygen-containing gas and fuel gas.
Between a pair of dividing plate 28, plug a plurality of (for example eight) electrolyte membrane-electrode assembly 26 to form fuel cell 11.These eight electrolyte membrane-electrode assemblies 26 are concentric with the fuel gas feed path 30 that extend at the center of passing dividing plate 28.
For example in Fig. 3, each dividing plate 28 comprises carbon plate or the single metal plate of being made by for example stainless steel alloy.Dividing plate 28 has first small-diameter end portions (reacting gas feeding unit) 32.Fuel gas feed path 30 is passed the center of first small-diameter end portions 32 and is extended.First small-diameter end portions 32 is integrally formed with disk (hold assembly) 36 by a plurality of first bridges 34.These first bridges 34 extend radially outwardly with equal angles (at interval) from first small-diameter end portions 32.
Disk 36 and electrolyte membrane-electrode assembly 26 have roughly the same size.At the center of disk 36 or the upstream position that on the oxygen-containing gas flow direction, departs from disk 36 centers be formed for the fuel gas inlet 38 of fuel supplying gas.In the outer end of disk 36 (in the peripheral part of dividing plate 28) plate-like extending portion 40 is set.Plate-like extending portion 40 is outwards outstanding along the direction shown in the arrow B.
Each disk 36 comprises the fuel gas channel 46 that is used for along the surperficial fuel supplying gas of anode 24 on the surperficial 36a of its contact anode 24.As shown in Figure 5, fuel gas channel 46 is included in a plurality of cannelures (channel unit) 48a to 48f that is formed centrally together around fuel gas inlet 38 on the disk 36.The cannelure 48a of diameter minimum is connected to fuel gas inlet 38 by straight trough 50.It is big that the diameter of cannelure outwards becomes from cannelure 48a to cannelure 48f.Cannelure 48a to 48f is by linking together along the link slot 52 of the arranged alternate of direction shown in the arrow B on front side and rear side.
The cannelure 48f of diameter maximum is connected to discharge orifice (through hole) 54 at its front end place along direction shown in the arrow B.As described below, fuel gas inlet 38 is connected to fuel gas discharge channel 68 by means of cannelure 48a to 48f by discharge orifice 54.Annular projection 56 is set in the outer regions of each disk 36.Annular projection 56 closely contacts with the peripheral part of the anode 24 of electrolyte membrane-electrode assembly 26.
As shown in Figure 6, each disk 36 has the flat surfaces 36b that contacts with negative electrode 22.Fuel gas service duct 58 extends to first bridge 34 from first small-diameter end portions 32.Fuel gas service duct 58 is connected to fuel gas inlet 38 with fuel gas feed path 30.For example, fuel gas service duct 58 can form by etching.
As shown in Figure 3, passage component 60 for example is fixed on dividing plate 28 on the surface of negative electrode 32 by soldering or Laser Welding.Passage component 60 has flat pattern, and comprises second small-diameter end portions 62.Fuel gas feed path 30 is passed the center of second small-diameter end portions 62 and is extended.Eight second bridges 64 radially extend from second small-diameter end portions 62.Each second bridge 64 is fixed to dividing plate 28, extends to the surperficial 36b of disk 36 from first bridge 34, and covers fuel gas inlet 38 (see figure 7)s.
As Fig. 3 and shown in Figure 7, letdown tank parts 66 are fixed to the surperficial 36b of disk 36.Letdown tank parts 66 cover discharge orifice 54 and plate-like extending portion 40.In letdown tank parts 66, form the letdown tank 66a that is connected to discharge orifice 54.Form fuel gas discharge channel 68 by discharge orifice 54 and letdown tank 66a.
Fuel gas discharge channel 68 is located outside opening in the end of letdown tank parts 66.Distance H between the outer peripheral face of the end of letdown tank parts 66 and electrolyte membrane-electrode assembly 26 is defined as making can suitably avoid dividing plate 28 and electrolyte membrane-electrode assembly 26 to be subjected to the influence of the burning gases that the mixture by waste gas and oxygen-containing gas forms, and avoids them to be subjected to the influence of water.
Deformable resilient channels parts are set on the surperficial 36b of disk 36, for example conduct electricity mesh members 72.Conduction mesh members 72 is formed for along the oxygen-containing gas passage 70 of the surface supply oxygen-containing gas of negative electrode 22, and the mesh members 72 of wherein conducting electricity is arranged as with negative electrode 22 and closely contacts.For example can also using, the felt parts replace mesh members 72.
For example, mesh members 72 can be made and had a disc-shape by stainless steel wire rod.The thickness of mesh members 72 is defined as making that mesh members 72 can strain when the load that applies to mesh members 72 along stacking direction (direction shown in the arrow A).Mesh members 72 directly contacts with the surperficial 36b of disk 36, and has otch 72a, 72b as the space that passage component 60 and letdown tank parts 66 are set.
As shown in Figure 7, be furnished with the power generation region of the zone of mesh members 72 less than anode 24.The oxygen-containing gas passage 70 that is formed in the mesh members 72 is connected to oxygen-containing gas feed path (oxygen-containing gas feeding unit) 74.Oxygen-containing gas by electrolyte membrane-electrode assembly 26 inner periphery and the space between the inner periphery of disk 36 along the direction supply shown in the arrow B.Oxygen-containing gas feed path 74 is extended along stacking direction in each disk 36 and first bridge 34.
Between dividing plate 28, be provided for the insulating sealer 76 of sealed fuel gas feed path 30.For example, insulating sealer 76 can be made by mica material or ceramic material.The exhaust passage 78 that is used for fuel cell 11 is formed on the outside of disk 36.
As depicted in figs. 1 and 2, fuel battery 12 comprises end plate 80a, the 80b that is arranged on the opposed end place of fuel cell 11 along stacking direction.End plate 80a has roughly disc-shape.Annular section 82 is outstanding from the peripheral end of end plate 80a, forms groove 84 around annular section 82.In annular section 82, be formed centrally stud bump 86.Stud bump 86 is outstanding along the direction identical with annular section 82.In projection 86, form stepped hole 88.
Hole 90 and screwed hole 92 form and are positioned at projection 86 same imaginary circle on every side.Hole 90 and screwed hole 92 arranged alternate with the corresponding position of corresponding space that is formed on the oxygen-containing gas feed path 74 between first bridge 34 and second bridge 64, predetermined angular (at interval) simultaneously separates each other.The diameter of end plate 80b is greater than the diameter of end plate 80a.In addition, end plate 80a is a conductive plate.
Housing 18 comprises the first housing unit 96a of load-accommodating applying mechanism 21 and holds the second housing unit 96b of fuel battery 12.An end plate 80b and an insulating element are clipped between the first housing unit 96a and the second housing unit 96b.This insulating element is arranged on the sidepiece of the second housing unit 96b.Bonding part between the first housing unit 96a and the second housing unit 96b is fastening by bolt 98 and nut 100.End plate 80b plays the effect of gas shield, and it has prevented to enter load applying mechanism 21 from the thermal exhaust of element of fluid 19 or hot-air.
One termination of annular wall plate 102 is incorporated into the second housing unit 96b, and top board 104 is fixed to the other end of wallboard 102.Element of fluid 19 is symmetrical arranged about the central axis of fuel battery 12.Specifically, the roughly reformer 16 of cylindricality coaxial setting in the heat exchanger 14 of general toroidal.
Wallboard 106 is fixed to the groove 84 around the end plate 80a, thereby forms passage component 108.Heat exchanger 14 and reformer 16 are directly connected to passage component 108.Form chamber 108a in passage component 108, its middle chamber 108a is filled with the air by heat exchanger 14 heating temporarily.Hole 90 forms opening, is used for the air supply of interim filled chamber 108a is arrived fuel battery 12.
Fuel gas supply pipe 110 and reformed gas supply pipe 112 are connected to reformer 16.Fuel gas supply pipe 110 extends to the outside from top board 104.Reformed gas supply pipe 112 inserts in the stepped hole 88 of end plate 80a, and is connected to fuel gas feed path 30.
Air supply pipe 114 and blast pipe 116 are connected to top board 104.In housing 18, be provided with from 114 extensions of air supply pipe and by the passage 118 of heat exchanger 14 to passage component 108 direct openings, and another passage 120 that extends to blast pipe 116 from the exhaust passage 78 of fuel battery 12 through over-heat-exchanger 14.
Load applying mechanism 21 comprises the first fastening unit 122a and the second fastening unit 122b, the first fastening unit 122a is used for applying the first fastening load T1 near the zone of (or) around the fuel gas feed path 30, and the second fastening unit 122b is used for applying the second fastening load T2 to electrolyte membrane-electrode assembly 26.The second fastening load T2 is less than the first fastening load T1 (T1＞T2).
The first fastening unit 122a comprises the first short fastening bolt 124a that is screwed in the screwed hole 92 that forms along diagonal of end plate 80a.The first fastening bolt 124a extends along the stacking direction of fuel cell 11, and engages with the first pressing plate 126a.The first fastening bolt 124a also is arranged in the oxygen-containing gas feed path 74 of passing dividing plate 28 extensions.The first pressing plate 126a is formed by narrow boards, and engages to cover fuel gas feed path 30 with the center of dividing plate 28.
The second fastening unit 122b comprises the second long fastening bolt 124b that is screwed in the screwed hole 92 that forms along another diagonal of end plate 80a.The end of the second fastening bolt 124b extends through the second pressing plate 126b with curved outer.Nut 127 is assembled to the end of the second fastening bolt 124b.The second fastening bolt 124b also is arranged in the oxygen-containing gas feed path 74 of passing dividing plate 28 extensions.In the corresponding circular portion of the second pressing plate 126b, spring 128 and spring base 129 are set in the position corresponding with electrolyte membrane-electrode assembly 26 on the disk 36 of fuel cell 11.Spring 118 for example is a ceramics springs.
The operation of fuel cell system 10 will be described below.
As shown in Figure 3, when assembling fuel cell system 10, at first, with passage component 60 join to dividing plate 28 on the surface of negative electrode 22.Therefore, between dividing plate 28 and passage component 60, form the fuel gas service duct 58 that is connected with fuel gas feed path 30.Fuel gas service duct 58 is connected to fuel gas channel 46 (see figure 7)s by fuel gas inlet 38.
Letdown tank parts 66 join on the surperficial 36b of each disk 36.Therefore, discharge orifice 54 and letdown tank 66a link together and form fuel gas discharge channel 68.Annular insulating sealer 76 is set around fuel gas feed path 30 on each dividing plate 28.
Make dividing plate 28 in the following manner.Specifically, between a pair of dividing plate 28, plug eight electrolyte membrane-electrode assemblies 26 to form fuel cell 11.As shown in Figure 3 and Figure 4, electrolyte membrane-electrode assembly 26 is plugged between the surperficial 36b of the surperficial 36a of a dividing plate 28 and another dividing plate 28.Fuel gas inlet 38 roughly is positioned at the center of each anode 24.Between the surperficial 36b of dividing plate 28 and electrolyte membrane-electrode assembly 26, mesh members 72 is set.Two otch 72a, 72b of mesh members 72 are arranged on and passage component 60 and letdown tank parts 66 corresponding positions.
Pile up a plurality of fuel cells 11 along the direction shown in the arrow A, end plate 80a, 80b are located at the place, opposite end along stacking direction.As depicted in figs. 1 and 2, the first pressing plate 126a of the first fastening unit 122a is arranged on the center of fuel cell 11.
Under this state, will insert towards end plate 80a than the first short fastening bolt 124a and pass the first pressing plate 126a and end plate 80b.The front end of the first fastening bolt 124a is screwed into and is assembled in the screwed hole 92 of the diagonal formation of end plate 80a.The head of the first fastening bolt 124a engages with the first pressing plate 126a.The first fastening bolt 124a rotates to regulate the surface pressing of the first pressing plate 126a in screwed hole 92.Like this, in fuel battery 12, near the zone fuel gas feed path 30 applies the first fastening load T1.
Then, spring 128 and spring base 129 are aimed in the relevant position of disk 36 coaxially with electrolyte membrane-electrode assembly 26.The second pressing plate 126b of the second fastening unit 122b engages with the spring base 129 of an end that is arranged on spring 128.
Then, will pass the second pressing plate 126b and end plate 80b towards end plate 80a insertion than the second long fastening bolt 124b.The front end of the second fastening bolt 124b is screwed into and is assembled in the screwed hole 92 of another diagonal formation of end plate 80a.Nut 127 is assembled to the head of the second fastening bolt 124b.Therefore, by the threads engage state between the adjusting nut 127 and the second fastening bolt 124b, the elastic force by respective springs 128 applies the second fastening load T2 to electrolyte membrane-electrode assembly 26.
The end plate 80b of fuel battery 12 is clipped between the first housing unit 96a and the second housing unit 96b of housing 18.The first housing unit 96a and the second housing unit 96b are fixed together by bolt 98 and nut 100.Element of fluid 19 is installed among the second housing unit 96b.The wallboard 106 of element of fluid 19 attaches to the groove 84 around the end plate 80a.Therefore, between end plate 80a and wallboard 106, passage component 108 is set.
As shown in Figure 1, in fuel cell system 10,, supply water when needed from fuel gas supply pipe 110 fuel supplying (methane, ethane, propane etc.), and from air supply pipe 114 supply oxygen-containing gass (hereinafter referred is " air ").
Thereby being reformed, fuel produces fuel gas (hydrogen-containing gas) through reformer 16 time.Fuel gas is supplied to the fuel gas feed path 30 of fuel battery 12.Fuel gas moves along the stacking direction shown in the arrow A, by dividing plate 28 inflow fuel gas service ducts 58 (see figure 7)s of each fuel cell 11.
Fuel gas flows along the fuel gas service duct between first and second bridges 34,64 58, and flows into the fuel gas inlet 38 of disk 36.Thereby fuel gas is supplied to fuel gas channel 46 on each disk 36.Fuel gas inlet 38 is formed on the corresponding position, approximate centre position with the anode 24 of electrolyte membrane-electrode assembly 26.Therefore, fuel gas is supplied to the approximate centre zone of anode 24 from fuel gas inlet 38, and outwards flows from the central area of anode 24.
Specifically, as shown in Figure 5, fuel gas channel 46 comprises a plurality of cannelure 48a to 48f.At first, fuel gas is supplied to cannelure 48a by the straight trough 50 that is connected to fuel gas inlet 38.When fuel gas flowed through cannelure 48a, fuel gas outwards flowed by link slot 52 temporarily, was supplied to the cannelure 48b in the cannelure 48a outside then.Thereby fuel gas flows along cannelure 48b then.
In addition, the fuel gas that is fed to the cannelure 48c in the cannelure 48b outside by link slot 52 flows along other cannelure 48d to 48f by link slot 52, arrives discharge orifice 54 up to fuel gas.Therefore, fuel gas is from the outwards supply of approximate centre zone of anode 24.After consuming, fuel gas is by discharge orifice 54 dischargings.
As shown in Figure 7, the fuel gas of the consumption by discharge orifice 54 discharging move towards surperficial 36b, and inflow letdown tank 66a.Thereby the fuel gas of consumption flows along fuel gas discharge channel 68 on the direction shown in the arrow B.Then, the fuel gas of consumption is discharged into the outside from the outer end of letdown tank parts 66.
As shown in Figure 1, pass through the passage 118 of heat exchanger 14 from the air flows of air supply pipe 114, and flow into chamber 108a temporarily.The hole 90 of air flows by being connected to chamber 108a, and be supplied to the oxygen-containing gas feed path 74 of the approximate centre that is arranged on fuel cell 11.At this moment, in heat exchanger 14, as described later, pass through passage 120 because be discharged into the exhaust flow of exhaust passage 78, so before fuel cell 11, between air and exhaust, carry out heat exchange at air supply.Therefore, air is heated to the temperature of fuel cell of expectation in advance.
Space between the oxygen-containing gas that is supplied to oxygen-containing gas feed path 74 flows into electrolyte membrane-electrode assembly 26 along the direction shown in the arrow B inner periphery and the inner periphery of disk 36, mobile towards the oxygen-containing gas passage 70 that forms by mesh members 72 then.As shown in Figure 7, in oxygen-containing gas passage 70, oxygen-containing gas flows to neighboring (exterior domain of dividing plate 28) from inner periphery (central area of dividing plate 28), more particularly, flows to the other end from an end of the outer regions of the negative electrode 22 of electrolyte membrane-electrode assembly 26.
Therefore, in electrolyte membrane-electrode assembly 26, fuel gas flows to outer regions from the central area of anode 24, and oxygen-containing gas flows on a direction shown in the arrow B along the electrode surface of negative electrode 22.At this moment, oxonium ion flows to anode 24 by electrolyte 20, with electrochemical reaction effect generating down betwixt.
The exhaust (waste gas) that drains into corresponding electrolyte membrane-electrode assembly 26 outsides flows through exhaust passage 78 along stacking direction.When exhaust flow is passed through the passage 120 of heat exchanger 14, between exhaust and air, carry out heat exchange.Then exhaust is drained into (see figure 1) in the blast pipe 116.
In the first embodiment, as shown in Figure 5, fuel gas channel 46 has and is positioned at fuel gas inlet 38 and to the starting point of the center of electrolyte membrane-electrode assembly 26 opening.In addition, fuel gas channel 46 has the terminal point that is positioned at the position corresponding with the neighboring of electrolyte membrane-electrode assembly 26.At this destination county, fuel gas channel 46 is connected to discharge orifice 54, thereby the fuel gas that will consume in electrolyte membrane-electrode assembly 26 is from fuel gas channel 46 dischargings.
As shown in Figure 7, flow into the fuel gas discharge channel 68 that comprises the letdown tank 66a that is arranged on the letdown tank parts 66 from discharge orifice 54 exhaust gas discharged.Waste gas moves along the direction shown in the arrow B in fuel gas discharge channel 68, and waste gas with the position of the outside H spaced a predetermined distance from of peripheral part of dividing plate 28 and electrolyte membrane-electrode assembly 26 overflow (discharging) arrive the outside.
Therefore, the zone (conversion zone) that mixes of waste gas and reacted oxygen-containing gas obviously separates with the peripheral part of electrolyte membrane-electrode assembly 26 and dividing plate 28.Thereby, prevented electrolyte membrane-electrode assembly 26 and dividing plate 28 owing to form the hot combustion gas of waste gas and air mixture or owing to any reaction of burning gases is locally heated to high temperature.In addition, electrolyte membrane-electrode assembly 26 and dividing plate 28 not can with during reaction contact with water generates.
Therefore, can prevent reliably because the corrosion that causes of steam oxidation, thereby can improve the durability of dividing plate 28.In addition, can prevent the oxidation of electrolyte membrane-electrode assembly 26, particularly the oxidation of anode 24.So, can prevent the impaired or deterioration of performance of electrolyte membrane-electrode assembly 26.
In the first embodiment, as Fig. 3 and shown in Figure 7, on the surperficial 36a of each disk 36, annular projection 56 is set.Annular projection 56 closely contacts with the peripheral part of anode 24.Therefore, exhaust can not enter the peripheral part of anode 24.Thereby, can utilize no seal (do not have sealing) to prevent that reliable in structure anode 24 is owing to oxidation and deterioration.
The negative electrode 22 of electrolyte membrane-electrode assembly 26 contacts with mesh members 72.In this state, the member to fuel cell 11 applies along the load of the stacking direction shown in the arrow A.Because mesh members 72 deformabilitys, so mesh members 72 keeps closely contacting with negative electrode 22.
In this structure, can suitably be absorbed in issuable scale error or distortion when making electrolyte membrane-electrode assembly 26 or dividing plate 28 by the strain of mesh members 72.Thereby in the first embodiment, prevented issuable damage when the member of stacking fuel cells 11.Because the member of fuel cell 11 contacts with each other in a plurality of positions, so can improve the performance from fuel cell 11 current collections the time.
In addition, in the first embodiment, fuel gas feed path 30 is arranged in the oxygen-containing gas feed path 74 airtightly, and along baffle surface fuel gas service duct 58 is set.Therefore, fuel gas was heated by the hot oxygen-containing gas that has heated by heat exchange in heat exchanger 14 before consuming.Thereby can improve the heat efficiency.
In addition, exhaust passage 78 be arranged on dividing plate 28 around.Exhaust passage 78 is used to prevent the thermal radiation from dividing plate 28.In addition, fuel gas inlet 38 is arranged on the approximate centre of disk 36, perhaps is arranged on along the oxygen-containing gas flow direction and departs from the upstream position at the center of disk 36.Therefore, the center radial diffusion from fuel gas inlet 38 supplied fuel gases from anode 24.Thereby reaction uniformly smoothly takes place, can improve fuel availability whereby.
In addition, the zone that occupies of mesh members 72 is than the little (see figure 6) of power generation region of anode 24.Therefore, even exhaust flow to anode 24 from the outer ring of electrolyte membrane-electrode assembly 26, there is not power generation region in the neighboring relative along the neighboring with anode 24 of negative electrode 22 yet.Like this, the fuel consumption of circulation can obviously not increase, and can easily collect bigger electromotive force.Therefore improve current collection performance, and can realize favourable fuel availability.In addition, the present invention can be only by using mesh members 72 easily to implement as the resilient channels parts.Like this, structure of the present invention not only simply but also save cost.
Specifically, even (promptly at the less electrolyte membrane-electrode assembly 26 of working strength with thin electrolyte 20 and thin negative electrode 22, so-called support membrane type MEA) time, the stress that is applied to electrolyte 20 and negative electrode 22 by mesh members 72 also is appropriate, thereby has advantageously reduced the damage to electrolyte membrane-electrode assembly 26.
In addition, eight electrolyte membrane-electrode assemblies 26 are arranged around the centres of dividing plate 28.Therefore, because the overall dimensions of fuel cell 11 is less, so can avoid the influence of thermal deformation.
In the first embodiment, fuel gas channel 46 comprises a plurality of cannelure 48a to 48f that arrange concentrically with respect to one another, and wherein link slot 52 connects cannelure 48a to 48f at corresponding diagonal position.Yet the present invention is unrestricted in this regard.Can adopt various other shapes.For example, described groove can have spiral-shaped.
Can use fuel gas channel 46a to replace fuel gas channel 46, as shown in Figure 8.Fuel gas channel 46a comprises a plurality of cannelure 48a to 48f that arrange concentrically with respect to one another in the mode identical with fuel gas channel 46.In addition, cannelure 48f has the cutting part 49 as its end.The discharge orifice 54a, the 54b that are connected to fuel gas discharge channel 68 are respectively formed at the two ends of cannelure 48f.
Fig. 9 is the exploded perspective view of expression according to the fuel cell 140 of second embodiment of the invention.With indicate identical Reference numeral according to the identical composed component of the fuel cell 11 of first execution mode, and will omit detailed description to these features.And in the 3rd to the 6th execution mode described later, and indicate identical Reference numeral, and will omit detailed description to these features according to the identical composed component of the fuel cell 11 of first execution mode.
Fuel cell 140 has dividing plate 142, wherein forms oxygen-containing gas passage 144 on the surface of the faces cathode 22 of dividing plate 142.Oxygen-containing gas passage 144 forms (seeing Figure 10 and 11) by a plurality of projections 146 on the surperficial 36b that is formed on each disk 36.
Projection 146 is the solid portions that for example form by etching on surperficial 36b.The cross sectional shape of projection 146 can adopt different shape, for example rectangle, circle or triangle.The position of these projections 146 or density can change arbitrarily according to the flow regime and/or the fluid situations of oxygen-containing gas etc.
In second execution mode, effectively transmit by the projection 146 of disk 36 along the load of stacking direction.Therefore, fuel cell 140 can utilize less load to be stacked, thereby reduces the distortion of electrolyte membrane-electrode assembly 26 and dividing plate 142.
Projection 146 on the surperficial 36b of disk 36 forms solid portion by etching etc.Therefore, the shape of these projections 146, position and density can easily change arbitrarily according to the flow regime and/or the fluid situations of oxygen-containing gas, can realize that whereby the expectation of fuel gas is flowed.In addition because projection 146 forms solid portion, so projection 146 can not be out of shape, thereby load transmit by projection 146 reliably, therefore by projection 146 current collection effectively.
Figure 12 is the exploded perspective view of expression according to the fuel cell 160 of third embodiment of the invention.
Fuel cell 160 has dividing plate 162, wherein forms fuel gas discharge channel 164 on the surface of anode 24 facing of dividing plate 162.Shown in Figure 12 and 13, fuel gas discharge channel 164 is formed on the surperficial 36a of each disk 36.Fuel gas discharge channel 164 comprises: letdown tank 166, and it is connected to fuel gas channel 46; And cover 168, thereby it is arranged on the last letdown tank 166 of closing of surperficial 36a.
Letdown tank 166 is set replaces discharge orifices 54, be arranged on along the corresponding position of plate-like extending portion 40 and discharge orifice 54.Letdown tank 166 comprises the step (not shown), and its middle cover assembly 168 is arranged on this step.Thereby the surface of the surface of cover 168 and annular projection 56 all is arranged in the same plane.
In the 3rd execution mode, as shown in figure 14, fuel gas flows through fuel gas channel 46, and is supplied to the anode 24 of electrolyte membrane-electrode assembly 26.After fuel gas during reaction consumed, fuel gas flowed near the letdown tank 166 anode 24 outer circumference end, and discharged along fuel gas discharge channel 164 on the direction shown in the arrow B.
Therefore, fuel gas is being overflowed with the position of the outside H spaced a predetermined distance from of peripheral part of electrolyte membrane-electrode assembly 26 after consuming.Thereby can obtain the advantage identical with first and second execution modes.For example, can prevent the damage or the deterioration of dividing plate 162 or electrolyte membrane-electrode assembly 26.
In first to the 3rd execution mode, outwards supply from the center of dividing plate 28,142,162 as the air of oxygen-containing gas.Yet the present invention is unrestricted in this regard.Optionally, air can be supplied in the lateral of dividing plate 28,142,162.
Figure 15 is the exploded perspective view of expression according to the fuel cell 180 of four embodiment of the invention.
Fuel cell 180 comprises dividing plate 182, wherein forms fuel gas channel 46 on the surface of anode 24 facing of dividing plate 182.Fuel gas channel 46 forms (seeing Figure 15 and 16) by a plurality of projections 186 on the surperficial 36a that is arranged on each disk 36.Projection 186 is for example to be formed on solid portion on the surperficial 36a by etching.
Figure 17 is the exploded perspective view of expression according to the fuel cell 190 of fifth embodiment of the invention.
Fuel cell 190 has dividing plate 192, and the deformable resilient channels parts such as conduction mesh members 196 wherein are set on the surperficial 36a of the disk 36 of dividing plate 192.Conduction mesh members 196 forms fuel gas channel 46, and fuel gas is by the surface supply of fuel gas channel 46 along anode 24, and the mesh members 196 of wherein conducting electricity closely contacts (seeing Figure 17 and 18) with anode 24.
Figure 19 is the stereogram that schematically shows according to the fuel battery 202 of sixth embodiment of the invention, and fuel battery 202 is by forming along the direction stacking fuel cells 200 shown in the arrow A.
As shown in figure 20, fuel cell 200 is established electrolyte membrane-electrode assembly 26 and is formed by folder between a pair of dividing plate 204.Each dividing plate 204 comprises first plate 206, second plate 208 and the 3rd plate 210.For example, first to the 3rd plate the 206,208, the 210th, for example metallic plate that forms by unoxidizable alloy.First plate 206 and the 3rd plate 210 for example join on two surfaces of second plate 208 by soldering.
Shown in Figure 20 and 21, first plate 206 has first small-diameter end portions (reacting gas feeding unit) 212.Be used for extending through first small-diameter end portions 212 along the fuel gas feed path 30 of the direction fuel supplying gas shown in the arrow A.First small-diameter end portions 212 is integrally formed by relatively large first disk (hold assembly) 216 of narrow bridge 214 and diameter.First disk 216 of electrolyte membrane-electrode assembly 26 and the size of anode 24 are roughly the same.
On first disk 216 and surface that anode 24 contacts, in the central area of contiguous outer regions, form the first a large amount of projections 220.The projection 222 of general toroidal is set on the outer regions of first disk 216.First projection 220 contacts with the anode 24 of electrolyte membrane-electrode assembly 26, thereby is formed for fuel gas is fed to the fuel gas channel 46 of anode 24 between first projection 220 and anode 24.First projection 220 and the general toroidal projection 222 common current-collectors that form.
Fuel gas inlet 38 is arranged on the center of first disk 216, is used for towards the approximate centre zone of anode 24 fuel supplying gas.In the general toroidal projection 222 of first disk 216, form a plurality of discharge orifices (through hole) 224.First projection 220 can form by being arranged on a plurality of recesses that surface with general toroidal projection 222 is arranged in conplane surface.A plurality of plate-like extending portion 226 at a predetermined angle (at interval) be arranged in the peripheral part of first disk 216.
As shown in figure 20, the 3rd plate 210 comprises second small-diameter end portions (reacting gas feeding unit) 228.Be used for extending through second small-diameter end portions 228 along the oxygen-containing gas feed path 74 of the supply of the direction shown in arrow A oxygen-containing gas.Second small-diameter end portions 228 is integrally formed by relatively large second disk (hold assembly) 232 of narrow bridge 230 and diameter.
As shown in figure 22, on second disk 232 and whole surface that negative electrode 22 electrolyte membrane-electrode assembly 26 contacts, form a plurality of second projections 234.Second projection 234 contacts with the negative electrode 22 of electrolyte membrane-electrode assembly 26, thereby is formed for oxygen-containing gas is fed to the oxygen-containing gas passage 70 of negative electrode 22 between second projection 234 and negative electrode 22.Second projection 234 plays the effect of current-collector.Oxygen-containing gas inlet 236 is arranged on the center of second disk 232, is used for the approximate centre zone supply oxygen-containing gas towards negative electrode 22.
As shown in figure 20, second plate 208 comprises the 3rd small-diameter end portions (reacting gas feeding unit) the 238 and the 4th small-diameter end portions (reacting gas feeding unit) 240.Fuel gas feed path 30 extends through the 3rd small-diameter end portions 238, and oxygen-containing gas feed path 74 extends through the 4th small-diameter end portions 240.It is integrally formed that third and fourth small-diameter end portions 238,240 is passed through relatively large the 3rd disk (hold assembly) 246 of narrow bridge 242,244 and diameter respectively.The diameter of first to the 3rd disk 216,232,246 is identical.
Along the peripheral part of the 3rd disk 246 at a predetermined angle (at interval) a plurality of plate-like extending portion 248 are set.When the first and the 3rd disk 216,246 was stacked, plate-like extending portion 226,248 formed the tubulose of essentially rectangular, and the fuel gas discharge channel 250 that wherein is connected to discharge orifice 224 is formed between the plate-like extending portion 226,248 (seeing Figure 22).
Fuel gas service duct 58 is formed between the bridge 214,242, and oxygen-containing gas service duct 252 is formed between the bridge 230,244.Oxygen-containing gas service duct 252 is connected to oxygen-containing gas inlet 236.
In the face of in the surface of first plate 206 separator 254 is set at the 3rd disk 246.Separator 254 is with respect to the center coaxial arrangement of the 3rd disk 246.Separator 254 is formed by the general toroidal projection, and wherein fuel gas service duct 58 is separated part 254 and is divided into the first and second fuel gas channel unit 58a, 58b.A plurality of the 3rd projections 256 are set on the surface of the 3rd disk 246 in separator 254 inboards.
As shown in figure 22, first plate 206 by soldered joint to second plate 208, thereby form fuel gas service duct 58, fuel gas service duct 58 is connected to fuel gas feed path 30 and fuel gas inlet 38 between first and second plates 206,208.
When fuel gas was fed to the first fuel gas channel unit 58a, first disk 216 contacted with anode 24 under pressure.Specifically, the first fuel gas channel unit 58a forms the first fuel gas pressure chamber 258a.The second fuel gas channel unit 58b is set around the first fuel gas pressure chamber 258a.When fuel gas is fed to the second fuel gas channel unit 58b, first disk 216 extrusion anode 24 under pressure.Specifically, the second fuel gas channel unit 58b forms the second fuel gas pressure chamber 258b.
Second plate 208 is by soldered joint to the three plates 210, thus formation oxygen-containing gas service duct 252, and oxygen-containing gas service duct 252 is connected to oxygen-containing gas feed path 74 and oxygen-containing gas inlet 236 between second plate 208 and the 3rd plate 210.When oxygen-containing gas was fed to oxygen-containing gas service duct 252, second disk 232 contacted with negative electrode 22 under pressure.Specifically, oxygen-containing gas service duct 252 forms oxygen-containing gas pressure chamber 260.As shown in figure 20, between dividing plate 204, plug insulating sealer 76a, 76b around fuel gas feed path 30 and oxygen-containing gas feed path 74.
As shown in figure 19, fuel battery 202 comprises end plate 270a, the 270b that is arranged on the opposed end place of fuel cell 200 along stacking direction.End plate 270a or end plate 270b and fastening bolt 272 electric insulations.First pipe, 274 and second pipe 276 extends through end plate 270a.First manages the oxygen-containing gas feed path 74 that 274 fuel gas feed path 30, the second pipes 276 that are connected to fuel cell 200 are connected to fuel cell 200.
In fuel battery 202, fuel gas is fed to first pipe 274 that links to each other with end plate 270a, and fuel gas flows into fuel gas feed path 30 from first pipe 274.Oxygen-containing gas (hereinafter referred is an air) is fed to second pipe 276 that links to each other with end plate 270a, and air flow to oxygen-containing gas feed path 74 from second pipe 276.
As shown in figure 22, after fuel gas flowed into fuel gas feed path 30, fuel gas flowed along the stacking direction shown in the arrow A, and was fed to the fuel gas service duct 58 in the dividing plate 204 of each fuel cell 200.Fuel gas flows along fuel gas service duct 58, flows into the first fuel gas channel unit 58a then.Fuel gas inlet 38 is formed on the center of the first fuel gas channel unit 58a.Fuel gas flows into fuel gas inlet 38 and flows to fuel gas channel 46.
After air flowed into oxygen-containing gas feed path 74, oxygen-containing gas flowed through the oxygen-containing gas service duct 252 in the dividing plate 28, and is fed to oxygen-containing gas pressure chamber 260.Air roughly flows into oxygen-containing gas inlet 236 at the center of second disk 232.
In each electrolyte membrane-electrode assembly 26, oxygen-containing gas inlet 236 is arranged on the position corresponding with the center of negative electrode 22.Therefore, as shown in figure 22, to oxygen-containing gas passage 70, and flow to the outer regions of negative electrode 22 from the central area of negative electrode 22 from the air supply of oxygen-containing gas inlet 236.
Thereby in each electrolyte membrane-electrode assembly 26, fuel gas is fed to the outer regions of anode 24 from the central area of anode 24, and air is fed to the outer regions of negative electrode 22 from the central area of negative electrode 22, thus generating.After fuel gas and air had consumed owing to generating, fuel gas and air entered in the exhaust passage 78 as exhaust.
In the 6th execution mode, fuel gas channel 46 has and is positioned at fuel gas inlet 38 and in the starting point of the central opening of electrolyte membrane-electrode assembly 26, in addition, fuel gas channel 46 has the terminal point that is positioned at general toroidal projection 222 places, is positioned at the position corresponding with the outer regions of electrolyte membrane-electrode assembly 26.The terminal point of fuel gas channel 46 is connected to discharge orifice 224, thereby the fuel gas that will consume in electrolyte membrane-electrode assembly 26 is from fuel gas channel 46 dischargings.
The waste gas that is disposed in the discharge orifice 224 flows into the fuel gas discharge channel 250 that forms between plate-like extending portion 226,248.Waste gas moves through discharge-channel 250 along the direction shown in the arrow B.Waste gas is from overflowing with the outside position spaced apart by a predetermined distance of the peripheral part of dividing plate 204 and electrolyte membrane-electrode assembly 26.
Therefore, the zone (conversion zone) that mixes of waste gas and reacted oxygen-containing gas obviously outwards separates with the peripheral part of electrolyte membrane-electrode assembly 26 and dividing plate 204.Thereby, can obtain and the identical advantage of first to the 5th execution mode.For example, electrolyte membrane-electrode assembly 26 and dividing plate 204 can be owing to constituting waste gas and Air mixing burning of gas gas or owing to any reaction of burning gases is locally heated to high temperature.Thereby can improve the durability of dividing plate 204.
Figure 23 is the exploded perspective view of expression according to the fuel cell 280 of seventh embodiment of the invention.With indicate identical Reference numeral according to the identical composed component of the fuel cell 200 of the 6th execution mode, thereby will omit description of them.
Fuel cell 280 has the dividing plate 282 that comprises first to the 3rd plate 284,286,210.First plate 284 and second plate 286 have ring-shaped skirt 288,290, replace the plate-like extending portion 226,248 that is provided with in the 6th execution mode.
Preset distance is outwards given prominence to from the outer end of the first and the 3rd disk 216,246 in skirt section 288,290, and forms fuel gas discharge channel 292 between skirt section 288,290.Thereby in the 7th execution mode, can obtain the advantage identical with the 6th execution mode.

Claims (23)

1. one kind by piling up electrolyte membrane-electrode assembly (26) and dividing plate (28,142,182,192) fuel cell (11 that forms, 140,180,190), described electrolyte membrane-electrode assembly (26) comprise anode (24), negative electrode (22) and be plugged in described anode (24) and described negative electrode (22) between electrolyte (20), described fuel cell (11,140,180,190) comprising:
Fuel gas channel (46), this fuel gas channel are formed on the surface of described dividing plate (28,142,182,192), and are used for the surperficial fuel supplying gas along described anode (24); And
Oxygen-containing gas passage (70,144), this oxygen-containing gas passage is formed on another surface of described dividing plate (28,142,182,192), and is used for the surface supply oxygen-containing gas along described negative electrode (22);
Wherein said fuel gas channel (46) has the terminal point that is positioned at the position corresponding with the peripheral part of described electrolyte membrane-electrode assembly (26), and this terminal point of wherein said fuel gas channel (46) is connected to fuel gas discharge channel (68), and this fuel gas discharge channel is used for making the fuel gas that consumes at described electrolyte membrane-electrode assembly (26) from overflowing with the outside position spaced of the peripheral part of described electrolyte membrane-electrode assembly (26); And
Wherein said fuel gas discharge channel (68) comprises the described dividing plate (28 of perforation, 142,182,192) through hole of Yan Shening (54), and be arranged on described dividing plate (28,142,182,192) the lip-deep letdown tank parts of another (66), described letdown tank parts (66) are connected to described through hole (54) and stretch out from described electrolyte membrane-electrode assembly (26).
2. fuel cell according to claim 1, wherein, described fuel gas channel (46) comprises a lip-deep channel unit (48a) that is arranged on described dividing plate (28), and this channel unit (48a) is connected to described fuel gas discharge channel (68) from the fuel gas inlet (38) to described fuel gas channel (46) fuel supplying gas.
3. fuel cell according to claim 1 wherein, is provided with the annular projection (56) that closely contacts with the peripheral part of described anode (24) on a surface of described dividing plate (28).
4. fuel cell according to claim 2, wherein, described channel unit comprises a groove (48a).
5. fuel cell according to claim 2, wherein, described channel unit comprises a plurality of projections (186).
6. fuel cell according to claim 2, wherein, described channel unit comprises the deformable elastic passage component of arranging in intimate contact with described anode (24) (196).
7. fuel cell according to claim 1, wherein, the deformable elastic passage component (72) that described oxygen-containing gas passage (70) comprises that another surface that is arranged on described dividing plate (28) is gone up and closely contacts with described negative electrode (22).
8. fuel cell according to claim 7 wherein, is arranged the power generation region of the zone of described resilient channels parts (72) less than described anode (24).
9. fuel cell according to claim 8, wherein, described resilient channels parts comprise in conduction mesh members (72) and the felt parts.
10. fuel cell according to claim 1, wherein, described oxygen-containing gas passage (144) comprises another lip-deep a plurality of projections (146) that are arranged on described dividing plate (142).
11. fuel cell according to claim 10, wherein, described projection (146) is included in another surface of described dividing plate (142) and goes up a plurality of solid portions that form by etching.
12. fuel cell according to claim 2, this fuel cell also comprises:
Fuel gas and oxygen-containing gas that exhaust passage (78), this exhaust passage are used for consuming at described electrolyte membrane-electrode assembly (26) between the stage of reaction discharge as the stacking direction of exhaust along described electrolyte membrane-electrode assembly (26) and described dividing plate (28);
Oxygen-containing gas feeding unit (74), this oxygen-containing gas feeding unit is used for oxygen-containing gas is fed to described oxygen-containing gas passage (70) along described stacking direction as the path of oxygen-containing gas before consuming; And
The fuel gas service duct (58) that is provided with is gone up on a surface or another surface at described dividing plate (28), described fuel gas service duct (58) is connected to the fuel gas feeding unit (32) as the path of fuel gas before consuming, and be connected to described fuel gas inlet (38)
Wherein said fuel gas feeding unit (32) is arranged in the described oxygen-containing gas feeding unit (74) airtightly, and
Wherein said fuel gas service duct (58) connects described fuel gas channel (46) and described fuel gas feeding unit (32), thereby and crossing with the described oxygen-containing gas feeding unit (74) that extends along described stacking direction along the surface arrangement of described dividing plate.
13. fuel cell according to claim 12, wherein, described exhaust passage (78) are arranged on described dividing plate (28) on every side.
14. fuel cell according to claim 12, wherein, described fuel gas feeding unit (32) is arranged on the core of described dividing plate (28) airtightly, and described oxygen-containing gas feeding unit (74) is arranged in the interior zone of described dividing plate (28).
15. fuel cell according to claim 12, wherein, described fuel gas inlet (38) is arranged on the core of described electrolyte membrane-electrode assembly (26).
16. fuel cell according to claim 1, wherein, described electrolyte membrane-electrode assembly (26) comprises a plurality of electrolyte membrane-electrode assemblies of arranging around the centres of described dividing plate (28).
17. one kind by piling up the fuel cell (200) that electrolyte membrane-electrode assembly (26) and dividing plate (204) form, described electrolyte membrane-electrode assembly (26) comprise anode (24), negative electrode (22) and be plugged in described anode (24) and described negative electrode (22) between electrolyte (20), described fuel cell (200) comprising:
Fuel gas channel (46), this fuel gas channel are formed on the surface of described dividing plate (204), and are used for the surperficial fuel supplying gas along described anode (24); And
Oxygen-containing gas passage (70), this oxygen-containing gas passage is formed on another surface of described dividing plate (204), and is used for the surface supply oxygen-containing gas along described negative electrode (22);
Wherein said fuel gas channel (46) has the terminal point that is positioned at the position corresponding with the peripheral part of described electrolyte membrane-electrode assembly (26), and this terminal point of wherein said fuel gas channel (46) is connected to fuel gas discharge channel (250), this fuel gas discharge channel is used for making the fuel gas that consumes at described electrolyte membrane-electrode assembly (26) from overflowing with the outside position spaced of the peripheral part of described electrolyte membrane-electrode assembly (26), wherein
Described fuel gas channel (46) comprises a lip-deep channel unit (48a) that is arranged on described dividing plate (204), this channel unit (48a) is connected to described fuel gas discharge channel (250) from the fuel gas inlet (38) to described fuel gas channel (46) fuel supplying gas
This fuel cell also comprises:
Fuel gas and oxygen-containing gas that exhaust passage (78), this exhaust passage are used for consuming at described electrolyte membrane-electrode assembly (26) between the stage of reaction discharge as the stacking direction of exhaust along described electrolyte membrane-electrode assembly (26) and described dividing plate (204); And
Oxygen-containing gas feeding unit (240), this oxygen-containing gas feeding unit is used for oxygen-containing gas is fed to described oxygen-containing gas passage (70) along described stacking direction as the path of oxygen-containing gas before consuming,
Wherein fuel gas feeding unit (238) and described oxygen-containing gas feeding unit (240) are arranged in the described exhaust passage (78) airtightly,
Wherein fuel gas service duct (58) connects described fuel gas channel (46) and described fuel gas feeding unit (238), thereby and crossing along the surface arrangement of described dividing plate with the described exhaust passage (78) of extending along described stacking direction, and
Wherein said oxygen-containing gas service duct (252) connects described oxygen-containing gas passage (70) and described oxygen-containing gas feeding unit (240), thereby and crossing with described exhaust passage (78) along the surface arrangement of described dividing plate.
18. fuel cell according to claim 17, wherein, described fuel gas channel (46) forms fuel gas pressure chamber (258a), make and when fuel gas is fed to described fuel gas channel (46), push described anode (24), and
Described oxygen-containing gas passage (70) forms oxygen-containing gas pressure chamber (260), makes and push described negative electrode (22) when described oxygen-containing gas is fed to described oxygen-containing gas passage (70).
19. one kind by piling up the fuel cell (11) that electrolyte membrane-electrode assembly (26) and dividing plate (28) form, described electrolyte membrane-electrode assembly (26) comprise anode (24), negative electrode (22) and be plugged in described anode (24) and described negative electrode (22) between electrolyte (20)
Described dividing plate (28) comprising:
Hold assembly (36), the described electrolyte membrane-electrode assembly of this hold assembly clamping (26), and have and be used for along the fuel gas inlet (38) of the surperficial fuel supplying gas of described anode (24) or be used for along the oxygen-containing gas inlet of the surface supply oxygen-containing gas of described negative electrode (22);
Bridge (34), this bridging are received described hold assembly (36), and have reacting gas service duct (58) therein, are used for fuel gas is fed to described fuel gas inlet (38), perhaps are used for oxygen-containing gas is fed to described oxygen-containing gas inlet; And
Reacting gas feeding unit (32), this reacting gas feeding unit one is connected to described bridge (34), and has reacting gas feed path (30) therein, be used for fuel gas or oxygen-containing gas are fed to described reacting gas service duct (58),
Fuel arranged gas discharge channel (68) in described hold assembly (36) wherein, this fuel gas discharge channel (68) is connected to fuel gas channel (46), is used for making the fuel gas that consumes at described electrolyte membrane-electrode assembly (26) from overflowing with the outside position spaced of the peripheral part of this electrolyte membrane-electrode assembly (26); And
Described fuel gas discharge channel (68) comprises the through hole (54) that connects described dividing plate (28) extension, and another lip-deep letdown tank parts (66) that are arranged on described dividing plate (28), described letdown tank parts (66) are connected to described through hole (54) and stretch out from described electrolyte membrane-electrode assembly (26).
20. one kind by piling up the fuel battery that a plurality of fuel cells (11) form, described fuel cell (11) is all by piling up electrolyte membrane-electrode assembly (26) and dividing plate (28) forms, described electrolyte membrane-electrode assembly (26) comprise anode (24), negative electrode (22) and be plugged in described anode (24) and described negative electrode (22) between electrolyte (20), described fuel battery comprises:
Fuel gas channel (46), this fuel gas channel are formed on the surface of described dividing plate (28), and are used for the surperficial fuel supplying gas along described anode (24); And
Oxygen-containing gas passage (70), this oxygen-containing gas passage is formed on another surface of described dividing plate (28), and is used for the surface supply oxygen-containing gas along described negative electrode (22);
Wherein said fuel gas channel (46) has the terminal point that is arranged in the position corresponding with the peripheral part of described electrolyte membrane-electrode assembly (26), the terminal point of described fuel gas channel (46) is connected to fuel gas discharge channel (68), and this fuel gas discharge channel makes the fuel gas that consumes in described electrolyte membrane-electrode assembly (26) from overflowing with the outside position spaced of the peripheral part of described electrolyte membrane-electrode assembly (26); And
Described fuel gas discharge channel (68) comprises the through hole (54) that connects described dividing plate (28) extension, and another lip-deep letdown tank parts (66) that are arranged on described dividing plate (28), described letdown tank parts (66) are connected to described through hole (54) and stretch out from described electrolyte membrane-electrode assembly (26).
21. fuel battery according to claim 20, wherein, on a surface of described dividing plate (28) or another surface, fuel gas service duct (58) is set, described fuel gas service duct (58) is connected to the fuel gas feeding unit (32) as the path of fuel gas before consuming, and is connected to fuel gas is fed to fuel gas inlet (38) in the described fuel gas channel (46).
22. one kind by piling up the fuel cell (160) that electrolyte membrane-electrode assembly (26) and dividing plate (162) form, described electrolyte membrane-electrode assembly (26) comprise anode (24), negative electrode (22) and be plugged in described anode (24) and described negative electrode (22) between electrolyte (20), described fuel cell (160) comprising:
Fuel gas channel (46), this fuel gas channel are formed on the surface of described dividing plate (162), and are used for the surperficial fuel supplying gas along described anode (24); And
Oxygen-containing gas passage (70), this oxygen-containing gas passage is formed on another surface of described dividing plate (162), and is used for the surface supply oxygen-containing gas along described negative electrode (22);
Wherein said fuel gas channel (46) has the terminal point that is positioned at the position corresponding with the peripheral part of described electrolyte membrane-electrode assembly (26), and this terminal point of wherein said fuel gas channel (46) is connected to fuel gas discharge channel (164), and this fuel gas discharge channel is used for making the fuel gas that consumes at described electrolyte membrane-electrode assembly (26) from overflowing with the outside position spaced of the peripheral part of described electrolyte membrane-electrode assembly (26); And
Wherein, described fuel gas discharge channel (164) comprising: letdown tank (166), this letdown tank are arranged on the surface of described dividing plate (162) and are connected to described fuel gas channel (46); And cover (168), this cover is arranged on the surface of described dividing plate (162) to cover described letdown tank (166).
23. fuel cell according to claim 22, wherein, described fuel gas channel (46) comprises a lip-deep channel unit (48a) that is arranged on described dividing plate (162), and this channel unit (48a) is connected to described fuel gas discharge channel (164) from the fuel gas inlet (38) to described fuel gas channel (46) fuel supplying gas.
CN2006800497836A 2005-12-28 2006-12-11 Fuel cell and fuel cell stack Expired - Fee Related CN101351917B (en)

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EP1969659A1 (en) 2008-09-17
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US20100221634A1 (en) 2010-09-02
KR101058771B1 (en) 2011-08-24
JP4611194B2 (en) 2011-01-12
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EP1969659B1 (en) 2011-10-19
US9401515B2 (en) 2016-07-26

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